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Template Guiding for the Encapsulation of Uniformly Subnanometric Platinum Clusters in Beta-Zeolites Enabling High Catalytic Activity and Stability
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2021-08-04 , DOI: 10.1002/anie.202108059
Yajie Tian 1, 2 , Haonan Duan 1 , Bofeng Zhang 3 , Siyuan Gong 3 , Zongjing Lu 3 , Lei Dai 2 , Congzhen Qiao 1 , Guozhu Liu 3 , Yong Zhao 2
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Subnanometric metal clusters have attracted extensive attention because of their unique properties as heterogeneous catalysts. However, it is challenging to obtain uniformly distributed metal clusters under synthesis and reaction conditions. Herein, we report a template-guidance protocol to synthesize subnanometric metal clusters uniformly encapsulated in beta-zeolite, with the metal ions anchored to the internal channels of the zeolite template via electrostatic interactions. Pt metal clusters with a narrow size range of 0.89 to 1.22 nm have been obtained on the intersectional sites of beta-zeolite (Pt@beta) with a broad range of Si/Al molar ratios (15–200). The uniformly distributed Pt clusters in Pt@H-beta are subject to strong electron withdrawal by the zeolite, which promotes transfer of active hydrogen, providing excellent activity and stability in hydrodeoxygenation reactions. A general strategy is thus proposed for the encapsulation of subnanometric metal clusters in zeolites with high thermal stability.

中文翻译:

用于在 β 沸石中包封均匀亚纳米铂簇的模板指南,可实现高催化活性和稳定性

亚纳米金属簇因其作为非均相催化剂的独特性质而受到广泛关注。然而,在合成和反应条件下获得均匀分布的金属簇具有挑战性。在此,我们报告了一种模板指导协议,用于合成均匀封装在 β 沸石中的亚纳米金属簇,金属离子通过静电相互作用固定在沸石模板的内部通道上。在具有宽范围的 Si/Al 摩尔比(15-200)的β-沸石(Pt@beta)的交叉位点上获得了尺寸范围为 0.89 至 1.22 nm 的窄 Pt 金属簇。Pt@H-beta 中均匀分布的 Pt 簇受到沸石的强吸电子作用,促进了活性氢的转移,在加氢脱氧反应中提供优异的活性和稳定性。因此,提出了一种通用策略,用于在具有高热稳定性的沸石中封装亚纳米金属簇。
更新日期:2021-09-20
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